Longitudinal magnetic field annealing is utilized for modifying the magnetic anisotropy and enhancing the magnetic softness of Fe75Co8(B10Si3C3P1)1-x/17Cux (x = 0.5, 0.75, 1, 1.25) nanocrystalline alloys. All of the magnetic field-annealed nanocrystalline alloys with Cu content more than 0.5 at.% exhibit significantly improved soft-magnetic properties, including high saturation magnetic flux density up to 1.87 T, effective permeability of 13,000–16,000 under the condition of 1 A/m and 1 kHz, coercivity as low as 1.6 A/m, and core loss of 0.11–0.45 W/kg under the condition of 1.0 T and 50 Hz. The application of a magnetic field promotes the nucleation and inhibits the growth of grains, leading to an increase in the number density of nanocrystals and the crystalline volume fraction, and a reduction in the grain size. The magnetic field annealing reduces the effective magneto-crystalline anisotropy energy to 2–4 J/m3, and induces longitudinal magnetic anisotropy with anisotropy energy density of 400–900 J/m3 which shows dependence on the crystalline volume fraction. The field-induced magnetic anisotropy dominates over the random local magnetic anisotropies, and results in the formation of regular magnetic domains aligned longitudinally, pinning-free domain wall displacement, and thus enhanced soft-magnetic properties.